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Liquid-Phase Epitaxially Grown Metal-Organic Framework Thin Films for Efficient Tandem Catalysis Through Site-Isolation of Catalytic Centers

机译:液相外延生长的金属 - 有机框架薄膜,通过催化中心的分离分离有效串联催化

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摘要

A functional metal-organic framework (MOF) composed of robust porphyrinic material (RPM) based on the pillared-paddlewheel topology is prepared with large 3D channels, and is used to perform a tandem epoxidation/CO2 insertion reaction. The designated system benefits from two metalloporphyrins: 1) a Mn-porphyrin, which catalyzes the epoxidation of an olefin substrate, and 2) a Zn-porphyrin, which catalyzes the epoxide opening. By using an automated liquid-phase epitaxial growth system, the RPM-MOF is also prepared in layer-by-layer fashion as an ultrathin film on a self-assembled-monolayer-coated silicon platform. Deployed as a tandem catalyst, the film version yields a substantially higher catalytic turnover number for tandem methoxy-styrene epoxidation followed by CO2 insertion than the bulk crystalline MOF samples.
机译:用大3D通道制备由基于柱状碎片拓扑的鲁棒卟啉材料(RPM)组成的功能金属 - 有机框架(MOF),并用于进行串联环氧化/ CO2插入反应。 指定的系统受益于两种金属卟啉:1)催化烯烃底物的环氧化,2)催化环氧化物开口的Mn-Porphylin。 通过使用自动液相外延生长系统,RPM-MOF也以层上的层式制备,作为自组装单层涂覆的硅平台上的超薄膜。 展开作为串联催化剂,薄膜版本产生串联甲氧基 - 苯乙烯环氧化的基本上更高的催化转换数,然后比散装晶体MOF样品涂抹于CO 2。

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